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Title: Steering CO 2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon

Abstract

Electrochemical reduction of CO 2 to multicarbon products is a significant challenge, especially for molecular complexes. We report here CO 2 reduction to multicarbon products based on a Ru(II) polypyridyl carbene complex that is immobilized on an N-doped porous carbon (RuPC/NPC) electrode. The catalyst utilizes the synergistic effects of the Ru(II) polypyridyl carbene complex and the NPC interface to steer CO 2 reduction toward C2 production at low overpotentials. In 0.5 M KHCO 3 /CO 2 aqueous solutions, Faradaic efficiencies of 31.0 to 38.4% have been obtained for C2 production at −0.87 to −1.07 V (vs. normal hydrogen electrode) with 21.0 to 27.5% for ethanol and 7.1 to 12.5% for acetate. Syngas is also produced with adjustable H 2 /CO mole ratios of 2.0 to 2.9. The RuPC/NPC electrocatalyst maintains its activity during 3-h CO 2 -reduction periods.

Authors:
; ; ; ; ; ; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1577930
Grant/Contract Number:  
SC0015739
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 52; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English

Citation Formats

Liu, Yanming, Fan, Xinfei, Nayak, Animesh, Wang, Ying, Shan, Bing, Quan, Xie, and Meyer, Thomas J. Steering CO 2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon. United States: N. p., 2019. Web. doi:10.1073/pnas.1907740116.
Liu, Yanming, Fan, Xinfei, Nayak, Animesh, Wang, Ying, Shan, Bing, Quan, Xie, & Meyer, Thomas J. Steering CO 2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon. United States. doi:10.1073/pnas.1907740116.
Liu, Yanming, Fan, Xinfei, Nayak, Animesh, Wang, Ying, Shan, Bing, Quan, Xie, and Meyer, Thomas J. Tue . "Steering CO 2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon". United States. doi:10.1073/pnas.1907740116.
@article{osti_1577930,
title = {Steering CO 2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon},
author = {Liu, Yanming and Fan, Xinfei and Nayak, Animesh and Wang, Ying and Shan, Bing and Quan, Xie and Meyer, Thomas J.},
abstractNote = {Electrochemical reduction of CO 2 to multicarbon products is a significant challenge, especially for molecular complexes. We report here CO 2 reduction to multicarbon products based on a Ru(II) polypyridyl carbene complex that is immobilized on an N-doped porous carbon (RuPC/NPC) electrode. The catalyst utilizes the synergistic effects of the Ru(II) polypyridyl carbene complex and the NPC interface to steer CO 2 reduction toward C2 production at low overpotentials. In 0.5 M KHCO 3 /CO 2 aqueous solutions, Faradaic efficiencies of 31.0 to 38.4% have been obtained for C2 production at −0.87 to −1.07 V (vs. normal hydrogen electrode) with 21.0 to 27.5% for ethanol and 7.1 to 12.5% for acetate. Syngas is also produced with adjustable H 2 /CO mole ratios of 2.0 to 2.9. The RuPC/NPC electrocatalyst maintains its activity during 3-h CO 2 -reduction periods.},
doi = {10.1073/pnas.1907740116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 52,
volume = 116,
place = {United States},
year = {2019},
month = {12}
}

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